Electrical Charge Coupling Dominates the Hysteresis Effect of Halide Perovskite Devices

Hysteresis effects in ionic-electronic devices are a valuable resource for the development of switching memory devices that can be used in information storage and brain-like computation. Halide perovskite devices show frequent hysteresis in current–voltage curves that can be harnessed to build effective memristors. These phenomena can be often described by a set of highly nonlinear differential equations that involve current, voltage, and internal state variables, in the style of the famous Hodgkin–Huxley model that accounts for the initiation and temporal response of action potentials in biological neurons. Here we extend the neuron-style models that lead to chemical inductors by introducing a capacitive coupling in the slow relaxation variable. The extended model is able to explain naturally previous observations concerning the transition from capacitor to inductor in impedance spectroscopy of MAPbBr solar cells and memristors in the dark. The model also generates new types of oscillating systems by the generation of a truly negative capacitance distinct from the usual inductive effect.

The author compares impedance spectra obtained by the model with measured ones from the literature.To validate the applicability of the proposed model, the author should fit the data with the proposed circuit, show the fit results, and quantitatively state the fit results.
The author shows that the model explains halide perovskites' complex and dynamic behaviour in the frequency domain.Is the same true for the time domain?I suggest adding units to the formula or the variables to allow the reader to follow equations easily.

Comments to the Author
The manuscript by Bisquert describes various equivalent circuit and extend the explanation towards neuron-style models that lead to chemical inductor by introducing a capacitive coupling.This is very interesting.
I have following suggestion or clarification to improve the manuscript.The presented model's are an attempt to unify the impedance response of perovskite material (MAPbBr).With the author extended model they explain naturally previous observations concerning the transition from capacitor to inductor in impedance spectroscopy up to 1.6V.
The text and title reflect persisting hysteresis effects in perovskites-but the analysis presented is in dark conditions, this does not truly support material behaviour, which are know to behave differently under light and heat condition.These claims can be verified better under light condition for accuracy and validation of results I will also suggest to modify the Abstract, and focus on MAPbBr as perovskites, as the text for the "development of switching memory devices that can be used in information storage and brain-like computation" is not supported in this work.
Since it is a single author article, I will also suggest to replace "we" with other word in conclusion section "In summary, we have complemented".Recommendation: This paper is publishable subject to minor revisions noted.Further review is not needed.

Comments:
The author proposes a model explaining halide perovskite devices' complex and dynamic behaviour.The model extends on known models of biological neurons and can explain the transition from the capacitor to inductor-like behaviour often observed in impedance spectroscopy of halide perovskites.The author finds that the timescales for capacitive and inductive effects are coupled, indicating that they originate from a single unified mechanism -which is an important finding.The results will be significant for moving forward using halide perovskites for resistive switches and memristors.I suggest the paper be published after minor revisions, as stated below.

I thank the reviewer for the positive comments
The author compares impedance spectra obtained by the model with measured ones from the literature.To validate the applicability of the proposed model, the author should fit the data with the proposed circuit, show the fit results, and quantitatively state the fit results.
Thanks for the suggestion.The data have been fitted and are shown as the new Fig. 4  and 5.
The author shows that the model explains halide perovskites' complex and dynamic behaviour in the frequency domain.Is the same true for the time domain?
The large scale perturbation techniques in the time domain are connected to the impedance results but the transformation is not straightforward.This topic has been discussed in Refs. 1,2.I have commented this point in the paper.I suggest adding units to the formula or the variables to allow the reader to follow equations easily.
I have added after Eq. ( 5): Note that units of and must be adjusted so that is in     amperes, in volts, in farads, and in seconds.   ,   In Fig. 1: and are in units of . ′ ′′ Ω

Reviewer: 2
Recommendation: This paper is probably publishable, but major revision is needed; I do not need to see future revisions.

Comments:
The manuscript by Bisquert describes various equivalent circuit and extend the explanation towards neuron-style models that lead to chemical inductor by introducing a capacitive coupling.This is very interesting.
Thank you for the positive comments.
I have following suggestion or clarification to improve the manuscript.Fig. 1 explain various circuit, while Fig. 2 and Fig. 3 are explanation based on published results and credit and ref. are given.Is the current article is a "research article" or "perspective" or "commentary"?Accordingly the text and abstract, and conclusion should be presented.
The paper introduces a new class of dynamical equations, Eqs.(4) (5).This is the new scientific contribution.Therefore I think this is an ordinary Letter paper.
The presented model's are an attempt to unify the impedance response of perovskite material (MAPbBr).With the author extended model they explain naturally previous observations concerning the transition from capacitor to inductor in impedance spectroscopy up to 1.6V.
The text and title reflect persisting hysteresis effects in perovskites-but the analysis presented is in dark conditions, this does not truly support material behaviour, which are know to behave differently under light and heat condition.These claims can be verified better under light condition for accuracy and validation of results The paper extracts conclusions from two previous papers 3,4 .These studies have been made in the dark because they enable to relate the behaviour of solar cells and memristors.

Fig. 1
Fig. 1 explain various circuit, while Fig.2 and Fig. 3 are explanation based on published results and credit and ref. are given.Is the current article is a "research article" or "perspective" or "commentary"?Accordingly the text and abstract, and conclusion should be presented.
Author's Response to Peer Review Comments: Journal: The Journal of Physical Chemistry Letters Manuscript ID: jz-2022-038128 Original Submission Date: 15-Dec-2022 Title: "Electrical Charge Coupling Dominates the Hysteresis Effect of Halide Perovskite Devices" Author(s): Bisquert, Juan Reviewer(s)' Comments to Author: Reviewer: 1